Synergistic water soluble preservative compositions of biocidal mixtures

ABSTRACT

A water soluble preservative admixture of biocidal compounds for addition to commercial use compositions at predetermined use levels, and uniformly distributed therein, to provide long-time synergistic biocidal activity against a wide range of fungi and both gram-negative and gram-positive bacteria, which comprises powders of (a) one or more methylol compounds, or their equivalents, and (b) iodopropynyl alcohol, or its ester, carbamate or ether derivative thereof, in a weight ratio of (a):(b) of 100:1 to 2000:1.

BACKGROUND OF THE INVENTION

1. Field of the Invention

This invention relates to a water soluble preservative admixture for addition to commercial use formulations to provide long time synergistic biocidal activity therein, and, more particularly, to admixtures of a methylol compound and an iodopropynyl compound, in predetermined weight ratios of 100:1 to 2000:1.

2. Description of the Prior Art

Combinations of antimicrobial agents have been developed in the prior art in order to:

(1) produce a biochemical synergism;

(2) broaden the antimicrobial spectrum of activity of each agent;

(3) increase water solubility for the admixture;

(4) minimize the toxicity or irritation of a given agent to the host; and

(5) minimize physical and chemical incompatibilities.

True biological synergism exists when two agents, when combined, require lesser amounts of the agents to bring about the same inhibitory or cidal effect than either single agent alone. While synergistic interaction for two or more antimicrobial agents does produce more than merely an additive effect in the resultant biological activity, in most cases the mechanism of such synergism remains a mystery.

M. Rosen et al., in U.S. Pat. No. 4,844,891, for example, described a preservative admixture of (a) a formaldehyde donor and (b) a halopropynyl compound, in a weight ratio of (a):(b) of 50:1 to 1:1, preferably 30:1 to 2:1, and, most preferably, 20:1 to 10:1, as providing fungicidal activity for 1-3 days in commercial use formulations. However, Rosen observed that when the ratio of (a):(b) in the concentrate exceeded 50:1 (System No. 16 in Table 1, a ratio of 73.33), the preservative composition was ineffective in providing biocidal protection in the use formulations. Thus a relatively large amount of the halopropynyl compound was required by Rosen to provide significant biocidal activity in the use composition. In such admixtures, although the formaldehyde donor is water soluble, the halopropynyl compound is substantially insoluble in water. Therefore it was difficult for Rosen to uniformly distribute his admixture throughout the use composition.

For these and other reasons, it is desired to provide a new and improved water soluble preservative admixture of such biocidal compounds which requires relatively little of the water insoluble and expensive halopropynyl compound, and that also provides effective synergistic protection in use formulations against a wide range of fungi and bacteria at different use levels over a long period of time.

A feature of the present invention is the provision of an admixture concentrate which is water soluble and which therefore can be uniformly distributed in use compositions at a predetermined use level.

Another feature herein is the provision of a preservative admixture which exhibits a long term synergistic biocidal activity against wide range of fungi and both gram-negative and gram-positive bacteria in the use compositions.

Still another feature of this invention is the provision of a water soluble preservative admixture for personal care compositions in the form of a solution, lotion, gel, emulsion, emulsifiable concentrate, suspension, slurry or cream.

These and other objects and features of the invention will be made apparent from the following more particular description of the invention.

SUMMARY OF THE INVENTION

What has been discovered is a water soluble preservative composition for addition to commercial use compositions at predetermined use levels, and uniformly distributed therein, which provides long term synergistic biocidal activity against a wide range of fungi and both gram-negative and gram-positive bacteria. The composition of the invention comprises an admixture of powders of

(a) a methylol compound, or their equivalent, and

(b) iodopropynyl alcohol, or its ester, carbamate or ether derivative thereof,

in a weight ratio of (a):(b) of 100:1 to 2000:1, preferably 200:1 to 500:1.

Commercial use compositions containing about 0.01 to 2% by weight of the composition of the invention also are provided therein. Such use compositions contain an iodopropynyl compound in an amount of about 0.5 to 10 ppm, to provide the desired antifungal activity, and a methylol compound, or equivalent thereof, in an amount of at least 250 ppm, to provide the desired antibacterial activity.

DETAILED DESCRIPTION OF THE INVENTION

The invention is based upon the discoveries that in a predetermined admixture of (a) a methylol compound, or its equivalent, and (b) an iodopropynyl compound:

(1) Iodopropynyl compounds are substantially water insoluble at weight ratios of (a):(b) of less than 100; accordingly, at weight ratios below 100:1, it is difficult to uniformly distribute the iodopropynyl compound in aqueous use compositions, particularly in creams, gels and the like. In this invention, the admixtures are used at a weight ratio of (a):(b) of 100:1 to 2000:1, which are water soluble in all use compositions at conventional use levels.

(2) Effective synergistic biocidal activity is achieved for admixtures having a weight ratio of (a):(b) of 100:1 to 2000:1. Such admixtures have a Synergistic Index (SI) value approaching zero (maximum synergism) for a wide range of organisms. In contrast, admixtures with (a):(b) ratios below 100:1, e.g. 10:1 to 50:1, are much less synergistic, and are active with only a narrower range of organisms.

(3) Preservative activity for use compositions is achieved most effectively with an admixture wt. ratio of 100:1 to 2000:1 at use levels of 0.05 to 2% by weight of the finished product. In this amount, the iodopropynyl compound is present in an amount of only 0.5-10 ppm, which significantly reduces the cost and toxicity of the use composition. The methylol compound also is present in an amount of at least 250 ppm.

The experimental results upon which these discoveries are based are described below. In these examples, the (a) methylol compound may be selected from diazolidinyl urea. (GERMALL® II) N-[1,3-bis (hydroxymethyl)-2,5-dioxo-4-imidazolidinyl]-N,N'-bis(hydroxymethyl) urea, imidurea (GERMALL® 115), 1,3-dimethylol-5,5-dimethyl hydantoin (DMDMH), sodium hydroxymethylglycinate (SUTTOCIDE® A), glycine anhydride dimethylol (GADM), dimethylhydroxymethyl pyrazole, (1-(3-chloroallyl)-3,5,7-triaza-1-azoniaadamantane chloride (a methylol equivalent),1,3,5-(trishydroxyethyl)hexahydrotriazine, or hydroxymethyl pyrrolidone; and the (b) iodopropynyl compound is iodopropynyl alcohol (IPGA) or 3-iodo-2-propynylbutyl carbamate (IPBC).

1. WATER SOLUBILITY

The water solubility or insolubility of admixtures of several methylol compounds with IPBC as 1% aqueous solutions is shown in Tables A through C below.

                  TABLE A                                                          ______________________________________                                         Weight Ratio of   Amount                                                       Germall ® II:IPBC                                                                            in ppm   Solubility                                          ______________________________________                                         2000:1             5       Soluble                                             1000:1             10      Soluble                                             500:1              20      Soluble                                             200:1              50      Soluble                                             100:1             100      Soluble                                              50:1             200      Insoluble                                            20:1             500      Insoluble                                           ______________________________________                                    

                  TABLE B                                                          ______________________________________                                         Weight Ratio of Amount                                                         GADM: IPBC      in ppm   Solubility                                            ______________________________________                                         2000:1           5       Soluble                                               1000:1          10       Soluble                                                500:1          20       Soluble                                                500:1          50       Soluble                                                100:1          100      Soluble                                                50:1           200      Insoluble                                              20:1           500      Insoluble                                             ______________________________________                                    

                  TABLE C                                                          ______________________________________                                         Weight Ratio of  Amount                                                        DMDMH: IPBC      in ppm   Solubility                                           ______________________________________                                         2000:1            5       Soluble                                              1000:1           10       Soluble                                              500:1            20       Soluble                                              200:1            50       Soluble                                              100:1            100      Soluble                                               50:1            200      Insoluble                                             20:1            500      Insoluble                                            ______________________________________                                    

These results demonstrate that admixtures having a ratio of 50:1 or 20:1 are insoluble in water whereas at ratios of 100:1 to 2000:1 the admixtures are soluble in water.

2. SYNERGISM

Tables 1 through 14 below demonstrate the very effective synergistic interaction between compounds "a" and "b" against a broad range of fungi and both gram-negative and gram-positive bacteria. The following organisms were tested:

    ______________________________________                                                      ATCC                                                              Organism     Number   Inoculum Concentration                                   ______________________________________                                         Ps. aeruginosa (PSA)*                                                                        9027    2.1 × 10.sup.6                                                                    CFU/gm of Product                               E. coli (ECOLI)*                                                                             8739    4.7 × 10.sup.5                                                                    CFU/gm of Product                               Staph. aureus (SA)**                                                                         6538    1.6 × 10.sup.6                                                                    CFU/gm of Product                               Ps. cepacia (PC)*                                                                           25416    1.6 × 10.sup.6                                                                    CFU/gm of Product                               C. albicans (CAN)***                                                                        10231    8.0 × 10.sup.4                                                                    CFU/gm of Product                               A. niger (AN)***                                                                            16404    2.7 × 10.sup.5                                                                    CFU/gm of Product                               ______________________________________                                    

                                      TABLE D                                      __________________________________________________________________________     Static (MIC) and Cidal Activities of Several Antimicrobial Compounds           (Static/Cidal Concentrations in ppm)                                           Organism (ATCC #)                                                                         IPBC  Germall ® II                                                                      GADM  DMDMH IPGA                                       __________________________________________________________________________     (SA) (6538)                                                                               100/200                                                                              400/1600                                                                              400/800                                                                              450/1600                                                                             300/5000                                   (ECOLI) (8739)                                                                             50/100                                                                              400/1600                                                                              400/800                                                                              400/800                                                                              150/600                                    (PSA) (9027)                                                                               800/1200                                                                            400/1600                                                                              400/400                                                                              600/1600                                                                             70/70                                      (PC) (25416)                                                                              1200/1800                                                                            200/400                                                                               200/400                                                                              600/1600                                                                             70/300                                     (CAN) (10231)                                                                              50/100                                                                              1500/15000                                                                             7500/15000                                                                          8000/16000                                                                           50/300                                     (AN) (16404)                                                                               50/100                                                                              3200/3200                                                                             1600/3200                                                                            8000/16000                                                                           30/30                                      __________________________________________________________________________

The Synergism Index was determined by the same mathematical treatment of such data described by Kull et al. in Applied Microbiology 9,538-541 (1961) using the following relationship: ##EQU1## where: 1. Q_(a) =The quantity of Compound a acting alone, producing an endpoint.

2. Q_(b) =The quantity of Compound b acting alone, producing and endpoint.

3. Q_(A) =The quantity of Compound A in mixture, producing an endpoint.

4. Q_(B) =The quantity of Compound in mixture, producing an endpoint.

When SI is equal to 1a mere additive effect of the components in the mixture is indicated; when SI is less than 1, synergism has occurred; and when SI is greater than 1 it indicates antagonism of the two components.

According to this well known method of measuring synergism, the quantity of each component in the various mixtures is compared with the, quantity of pure component that is required to reach the same endpoint or to produce the same microbiological effect as the mixture.

                  TABLE 1                                                          ______________________________________                                         2000:1 Wt. Ratio GERMALL ® II/IPBC                                         Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600  0.05  99.95  0.06                               "       ECOLI    100     1600  0.05  99.95  0.06                               "       PSA      1200    1600  0.05  99.95  0.06                               "       PC       1800    1250  0.05  99.95  0.08                               "       CAN      100     15000 0.05  99.95  0.01                               "       AN       100     3200  0.05  99.95  0.03                                0.025% SA       200     1600  0.125 249.9  0.16                               "       ECOLI    100     1600  0.125 249.9  0.16                               "       PSA      1200    1600  0.125 249.9  0.16                               "       PC       1800    1250  0.125 249.9  0.20                               "       CAN      100     15000 0.125 249.9  0.02                               "       AN       100     3200  0.125 249.9  0.08                               0.05%   SA       200     1600  0.25  499.8  0.31                               "       ECOLI    100     1600  0.25  499.8  0.31                               "       PSA      1200    1600  0.25  499.8  0.31                               "       PC       1800    1250  0.25  499.8  0.40                               "       CAN      100     15000 0.25  499.8  0.04                               "       AN       100     3200  0.25  499.8  0.16                               0.10%   SA       200     1600  0.5   999.5  0.63                               "       ECOLI    100     1600  0.5   999.5  0.63                               "       PSA      1200    1600  0.5   999.5  0.63                               "       PC       1800    1250  0.5   999.5  0.80                               "       CAN      100     15000 0.5   999.5  0.07                               "       AN       100     3200  0.5   999.5  0.32                               0.20%   SA       200     1600  1     1999   1.25                               "       ECOLI    100     1600  1     1999   1.26                               "       PSA      1200    1600  1     1999   1.25                               "       PC       1800    1250  1     1999   1.60                               "       CAN      100     15000 1     1999   0.14                               "       AN       100     3200  1     1999   0.63                               0.40%   SA       200     1600  2     3998   2.51                               "       ECOLI    100     1600  2     3998   2.52                               "       PSA      1200    1600  2     3998   2.50                               "       PC       1800    1250  2     3998   3.20                               "       CAN      100     15000 2     3998   0.29                               "       AN       100     3200  2     3998   1.27                               0.50%   SA       200     1600  2.5   4997.5 3.14                               "       ECOLI    100     1600  2.5   4997.5 3.15                               "       PSA      1200    1600  2.5   4997.5 3.13                               "       PC       1800    1250  2.5   4997.5 4.00                               "       CAN      100     15000 2.5   4997.5 0.36                               -       AN       100     3200  2.5   4997.5 1.59                               ______________________________________                                    

                  TABLE 2                                                          ______________________________________                                         1000:1 Wt. Ratio GERMALL ® II/IPBC                                         Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                               Q.sub.A                                                                             Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600   0.1  99.9   0.06                               "       ECOLI    100     1600   0.1  99.9   0.06                               "       PSA      1200    1600   0.1  99.9   0.06                               "       PC       1800    1250   0.1  99.9   0.08                               "       CAN      100     15000  0.1  99.9   0.01                               "       AN       100     3200   0.1  99.9   0.03                                0.025% SA       200     1600   0.25 249.8  0.16                               "       ECOLI    100     1600   0.25 249.8  0.16                               "       PSA      1200    1600   0.25 249.8  0.16                               "       PC       1800    1250   0.25 249.8  0.20                               "       CAN      100     15000  0.25 249.8  0.02                               "       AN       100     3200   0.25 249.8  0.08                               0.05%   SA       200     1600   0.5  499.5  0.31                               "       ECOLI    100     1600   0.5  499.5  0.32                               "       PSA      1200    1600   0.5  499.5  0.31                               "       PC       1800    1250   0.5  499.5  0.40                               "       CAN      100     15000  0.5  499.5  0.04                               "       AN       100     3200   0.5  499.5  0.16                               0.10%   SA       200     1600   1    999    0.63                               "       ECOLI    100     1600   1    999    0.63                               "       PSA      1200    1600   1    999    0.63                               "       PC       1800    1250   1    999    0.80                               "       CAN      100     15000  1    999    0.08                               "       AN       100     3200   1    999    0.32                               0.20%   SA       200     1600   2    1998   1.26                               "       ECOLI    100     1600   2    1998   1.27                               "       PSA      1200    1600   2    1998   1.25                               "       PC       isoo    1250   2    1998   1.60                               "       CAN      100     15000  2    1998   0.15                               "       AN       100     3200   2    1998   0.64                               0.40%   SA       200     1600   4    3996   2.52                               "       ECOLI    100     1600   4    3996   2.54                               "       PSA      1200    1600   4    3996   2.50                               "       PC       1800    1250   4    3996   3.20                               "       CAN      100     15000  4    3996   0.31                               "       AN       100     3200   4    3996   1.29                               0.50%   SA       200     1600   5    4995   3.15                               "       ECOLI    100     1600   5    4995   3.17                               "       PSA      1200    1600   5    4995   3.13                               "       PC       1800    1250   5    4995   4.00                               "       CAN      100     15000  5    4995   0.38                               "       AN       100     3200   5    4995   1.61                               ______________________________________                                    

                  TABLE 3                                                          ______________________________________                                         500:1 Wt. Ratio GERMALL ® II/IPBC                                          Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                               Q.sub.A                                                                             Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600   0.2  99.8   0.06                               "       ECOLI    100     1600   0.2  99.8   0.06                               "       PSA      1200    1600   0.2  99.8   0.06                               "       PC       1800    1250   0.2  99.8   0.08                               "       CAN      100     15000  0.2  99.8   0.01                               "       AN       100     3200   0.2  99.8   0.03                                0.025% SA       200     1600   0.5  249.5  0.16                               "       ECOLI    100     1600   0.5  249.5  0.16                               "       PSA      1200    1600   0.5  249.5  0.16                               "       PC       1800    1250   0.5  249.5  0.20                               "       CAN      100     15000  0.5  249.5  0.02                               "       AN       100     3200   0.5  249.5  0.08                               0.05%   SA       200     1600   1    499    0.32                               "       ECOLI    100     1600   1    499    0.32                               "       PSA      1200    1600   1    499    0.31                               "       PC       1800    1250   1    499    0.40                               "       CAN      100     15000  1    499    0.04                               "       AN       100     3200   1    499    0.17                               0.10%   SA       200     1600   2    998    0.63                               "       ECOLI    100     1600   2    998    0.64                               "       PSA      1200    1600   2    998    0.63                               "       PC       1800    1250   2    998    0.80                               "       CAN      100     15000  2    998    0.09                               "       AN       100     3200   2    998    0.33                               0.20%   SA       200     1600   4    1996   1.27                               "       ECOLI    100     1600   4    1996   1.29                               "       PSA      1200    1600   4    1996   1.25                               "       PC       1800    1250   4    1996   1.60                               "       CAN      100     15000  4    1996   0.17                               "       AN       100     3200   4    1996   0.66                               0.40%   SA       200     1600   8    3992   2.54                               "       ECOLI    100     1600   8    3992   2.58                               "       PSA      1200    1600   8    3992   2.50                               "       PC       1800    1250   8    3992   3.20                               "       CAN      100     15000  8    3992   0.35                               "       AN       100     3200   8    3992   1.33                               0.50%   SA       200     1600   10   4990   3.17                               "       ECOLI    100     1600   10   4990   3.22                               "       PSA      1200    1600   10   4990   3.13                               "       PC       1800    1250   10   4990   4.00                               "       CAN      100     15000  10   4990   0.43                               "       AN       100     3200   10   4990   1.66                               ______________________________________                                    

                  TABLE 4                                                          ______________________________________                                         200:1 Wt. Ratio GERMALL ® II/IPBC                                          Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                               Q.sub.A                                                                             Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600   0.5  99.5   0.06                               "       ECOLI    100     1600   0.5  99.5   0.07                               "       PSA      1200    1600   0.5  99.5   0.06                               "       PC       1800    1250   0.5  99.5   0.08                               "       CAN      100     15000  0.5  99.5   0.01                               "       AN       100     3200   0.5  99.5   0.04                                0.025% SA       200     1600   1.25 248.75 0.16                               "       ECOLI    100     1600   1.25 248.75 0.17                               "       PSA      1200    1600   1.25 248.75 0.16                               "       PC       1800    1250   1.25 248.75 0.20                               "       CAN      100     15000  1.25 248.75 0.03                               "       AN       100     3200   1.25 248.75 0.09                               0.05%   SA       200     1600   2.5  497.5  0.32                               "       ECOLI    100     1600   2.5  497.5  0.34                               "       PSA      1200    1600   2.5  497.5  0.31                               "       PC       1800    1250   2.5  497.5  0.40                               "       CAN      100     15000  2.5  497.5  0.06                               "       AN       100     3200   2.5  497.5  0.18                               0.10%   SA       200     1600   5    995    0.65                               "       ECOLI    100     1600   5    995    0.67                               "       PSA      1200    1600   5    995    0.63                               "       PC       1800    1250   5    995    0.80                               "       CAN      100     15000  5    995    0.12                               "       AN       100     3200   5    995    0.36                               0.20%   SA       200     1600   10   1990   1.29                               "       ECOLI    100     1600   10   1990   1.34                               "       PSA      1200    1600   10   1990   1.25                               "       PC       1800    1250   10   1990   1.60                               "       CAN      100     15000  10   1990   0.23                               "       AN       100     3200   10   1990   0.72                               0.40%   SA       200     1600   20   3980   2.59                               "       ECOLI    100     1600   20   3980   2.69                               "       PSA      1200    1600   20   3980   2.50                               "       PC       1800    1250   20   3980   3.20                               "       CAN      100     15000  20   3980   0.47                               "       AN       100     3200   20   3980   1.44                               0.50%   SA       200     1600   25   4975   3.23                               "       ECOLI    100     1600   25   4975   3.36                               "       PSA      1200    1600   25   4975   3.13                               "       PC       1800    1250   25   4975   3.99                               "       CAN      100     15000  25   4975   0.58                               "       AN       100     3200   25   4975   1.80                               ______________________________________                                    

                  TABLE 5                                                          ______________________________________                                         100:1 Wt. Ratio GERMALL ® II/IPBC                                          Use Level                                                                              Organism  Q.sub.a Q.sub.b                                                                               Q.sub.A                                                                             Q.sub.B                                                                              SI                                 ______________________________________                                         0.01%   SA        200     1600   1     99   0.06                               "       ECOLI     100     1600   1     99   0.07                               "       PSA       1200    1600   1     99   0.06                               "       PC        1800    1250   1     99   0.08                               "       CAN       100     15000  1     99   0.02                               "       AN        100     3200   1     99   0.04                                0.025% SA        200     1600   2.5   248  0.17                               "       ECOLI     100     1600   2.5   248  0.18                               "       PSA       1200    1600   2.5   248  0.16                               "       PC        1800    1250   2.5   248  0.20                               "       CAN       100     15000  2.5   248  0.04                               "       AN        100     3200   2.5   248  0.10                               0.05%   SA        200     1600   5     495  0.33                               "       ECOLI     100     1600   5     495  0.36                               "       PSA       1200    1600   5     495  0.31                               "       PC        1800    1250   5     495  0.40                               "       CAN       100     15000  5     495  0.08                               "       AN        100     3200   5     495  0.20                               0.10%   SA        200     1600   10    990  0.67                               "       ECOLI     100     1600   10    990  0.72                               "       PSA       1200    1600   10    990  0.63                               "       PC        1800    1250   10    990  0.80                               "       CAN       100     15000  10    990  0.17                               "       AN        100     3200   10    990  0.41                               0.20%   SA        200     1600   20   1980  1.34                               "       ECOLI     100     1600   20   1980  1.44                               "       PSA       1200    1600   20   1980  1.25                               "       PC        1800    1250   20   1980  1.60                               "       CAN       100     15000  20   1980  0.33                               "       AN        100     3200   20   1980  0.82                               0.40%   SA        200     1600   40   3960  2.68                               "       ECOLI     100     1600   40   3960  2.88                               "       PSA       1200    1600   40   3960  2.51                               "       PC        1800    1250   40   3960  3.19                               "       CAN       100     15000  40   3960  0.66                               "       AN        100     3200   40   3960  1.64                               0.50%   SA        200     1600   50   4950  3.34                               "       ECOLI     100     1600   50   4950  3.59                               "       PSA       1200    1600   50   4950  3.14                               "       PC        1800    1250   50   4950  3.99                               "       CAN       100     15000  50   4950  0.83                               "       AN        100     3200   50   4950  2.05                               ______________________________________                                    

                  TABLE 6                                                          ______________________________________                                         50:1 Wt. Ratio GERMALL ® II/IPBC                                           Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                              SI                                  ______________________________________                                         0.01%   SA       200     1600   2     98   0.07                                0.01%   ECOLI    100     1600   2     98   0.08                                0.01%   PSA      1200    1600   2     98   0.06                                0.01%   PC       1800    1250   2     98   0.08                                0.01%   CAN      100     15000  2     98   0.03                                0.01%   AN       100     3200   2     98   0.05                                 0.025% SA       200     1600   5    245   0.18                                 0.025% ECOLI    100     1600   5    245   0.20                                 0.025% PSA      1200    1600   5    245   0.16                                 0.025% PC       1800    1250   5    245   0.20                                 0.025% CAN      100     15000  5    245   0.07                                 0.025% AN       100     3200   5    245   0.13                                0.05%   SA       200     1600  10    490   0.36                                0.05%   ECOLI    100     1600  10    490   0.41                                0.05%   PSA      1200    1600  10    490   0.31                                0.05%   PC       1800    1250  10    490   0.40                                0.05%   CAN      100     15000 10    490   0.13                                0.05%   AN       100     3200  10    490   0.25                                0.10%   SA       200     1600  20    980   0.71                                0.10%   ECOLI    100     1600  20    980   0.81                                0.10%   PSA      1200    1600  20    980   0.63                                0.10%   PC       1800    1250  20    980   0.80                                0.10%   CAN      100     15000 20    980   0.27                                0.10%   AN       100     3200  20    980   0.51                                0.20%   SA       200     1600  40    1960  1.43                                0.20%   ECOLI    100     1600  40    1960  1.63                                0.20%   PSA      1200    1600  40    1960  1.26                                0.20%   PC       1800    1250  40    1960  1.59                                0.20%   CAN      100     15000 40    1960  0.53                                0.20%   AN       100     3200  40    1960  1.01                                0.40%   SA       200     1600  80    3920  2.85                                0.40%   ECOLI    100     1600  80    3920  3.25                                0.40%   PSA      1200    1600  80    3920  2.52                                0.40%   PC       1800    1250  80    3920  3.18                                0.40%   CAN      100     15000 80    3920  1.06                                0.40%   AN       100     3200  80    3920  2.03                                0.50%   SA       200     1600  100   4900  3.56                                0.50%   ECOLI    100     1600  100   4900  4.06                                0.50%   PSA      1200    1600  100   4900  3.15                                0.50%   PC       1800    1250  100   4990  3.98                                0.50%   CAN      100     15000 100   4900  1.33                                0.50%   AN       100     3200  100   4900  2.53                                ______________________________________                                    

                  TABLE 7                                                          ______________________________________                                         20:1 Wt. Ratio GERMALL ® II/IPBC                                           Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                             Q.sub.B                                                                               SI                                  ______________________________________                                         0.01%   SA       200     1600   5    95    0.08                                0.01%   ECOLI    100     1600   5    95    0.11                                0.01%   PSA      1200    1600   5    95    0.06                                0.01%   PC       1800    1250   5    95    0.08                                0.01%   CAN      100     15000  5    95    0.06                                0.01%   AN       100     3200   5    95    0.08                                 0.025% SA       200     1600    12.5                                                                                237.5                                                                               0.21                                 0.025% ECOLI    100     1600    12.5                                                                                237.5                                                                               0.27                                 0.025% PSA      1200    1600    12.5                                                                                237.5                                                                               0.16                                 0.025% PC       1800    1250    12.5                                                                                237.5                                                                               0.20                                 0.025% CAN      100     15000   12.5                                                                                237.5                                                                               0.14                                 0.025% AN       100     3200    12.5                                                                                237.5                                                                               0.20                                0.05%   SA       200     1600   25   475   0.42                                0.05%   ECOLI    100     1600   25   475   0.55                                0.05%   PSA      1200    1600   25   475   0.32                                0.05%   PC       1800    1250   25   475   0.39                                0.05%   CAN      100     15000  25   475   0.28                                0.05%   AN       100     3200   25   475   0.40                                0.10%   SA       200     1600   50   950   0.84                                0.10%   ECOLI    100     1600   50   950   1.09                                0.10%   PSA      1200    1600   50   950   0.64                                0.10%   PC       1800    1250   50   950   0.79                                0.10%   CAN      100     15000  50   950   0.56                                0.10%   AN       100     3200   50   950   0.80                                0.20%   SA       200     1600  100  1900   1.69                                0.20%   ECOLI    100     1600  100  1900   2.19                                0.20%   PSA      1200    1600  100  1900   1.27                                0.20%   PC       1800    1250  100  1900   1.58                                0.20%   CAN      100     15000 100  1900   1.13                                0.20%   AN       100     3200  100  1900   1.59                                0.40%   SA       200     1600  200  4800   4.00                                0.40%   ECOLI    100     1600  200  4800   5.00                                0.40%   PSA      1200    1600  200  4800   3.17                                0.40%   PC       1800    1250  200  4800   3.95                                0.40%   CAN      100     15000 200  4800   2.32                                0.40%   AN       100     3200  200  4800   3.50                                0.50%   SA       200     1600  250  4750   4.22                                0.50%   ECOLI    100     1600  250  4750   5.47                                0.50%   PSA      1200    1600  250  4750   3.18                                0.50%   PC       1800    1250  250  4750   3.94                                0.50%   CAN      100     15000 250  4750   2.82                                0.50%   AN       100     3200  250  4750   3.98                                ______________________________________                                    

                  TABLE 8                                                          ______________________________________                                         2000:1 Wt. Ratio DMDMH/IPBC                                                    Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                              SI                                  ______________________________________                                         0.01%   SA       200     1600  0.05   99.95                                                                               0.06                                0.01%   ECOLI    100      800  0.05   99.95                                                                               0.13                                0.01%   PSA      1200    1600  0.05   99.95                                                                               0.06                                0.01%   PC       1800    1600  0.05   99.95                                                                               0.06                                0.01%   CAN      100     16000 0.05   99.95                                                                               0.01                                0.01%   AN       100     16000 0.05   99.95                                                                               0.01                                 0.025% SA       200     1600   0.125                                                                               249.88                                                                               0.16                                 0.025% ECOLI    100      800   0.125                                                                               249.88                                                                               0.31                                 0.025% PSA      1200    1600   0.125                                                                               249.88                                                                               0.16                                 0.025% PC       1800    1600   0.125                                                                               249.88                                                                               0.16                                 0.025% CAN      100     16000  0.125                                                                               249.88                                                                               0.02                                 0.025% AN       100     16000  0.125                                                                               249.88                                                                               0.02                                0.05%   SA       200     1600  0.25  499.75                                                                               0.31                                0.05%   ECOLI    100      800  0.25  499.75                                                                               0.63                                0.05%   PSA      1200    1600  0.25  499.75                                                                               0.31                                0.05%   PC       1800    1600  0.25  499.75                                                                               0.31                                0.05%   CAN      100     16000 0.25  499.75                                                                               0.03                                0.05%   AN       100     16000 0.25  499.75                                                                               0.03                                0.10%   SA       200     1600  0.5   999.5 0.63                                0.10%   ECOLI    100      800  0.5   999.5 1.25                                0.10%   PSA      1200    1600  0.5   999.5 0.63                                0.10%   PC       1800    1600  0.5   999.5 0.62                                0.10%   CAN      100     16000 0.5   999.5 0.07                                0.10%   AN       100     16000 0.5   999.5 0.07                                0.20%   SA       200     1600  1     1999  1.25                                0.20%   ECOLI    100      800  1     1999  2.51                                0.20%   PSA      1200    1600  1     1999  1.25                                0.20%   PC       1800    1600  1     1999  1.25                                0.20%   CAN      100     16000 1     1999  0.13                                0.20%   AN       100     16000 1     1999  0.13                                0.40%   SA       200     1600  2     3998  2.51                                0.40%   ECOLI    100      800  2     3998  5.02                                0.40%   PSA      1200    1600  2     3998  2.50                                0.40%   PC       1800    1600  2     3998  2.50                                0.40%   CAN      100     16000 2     3998  0.27                                0.40%   AN       100     16000 2     3998  0.27                                0.50%   SA       200     1600  2.5   4997.5                                                                               3.14                                0.50%   ECOLI    100      800  2.5   4997.5                                                                               6.27                                0.50%   PSA      1200    1600  2.5   4997.5                                                                               3.13                                0.50%   PC       1800    1600  2.5   4997.5                                                                               3.12                                0.50%   CAN      100     16000 2.5   4997.5                                                                               0.34                                0.50%   AN       100     16000 2.5   4997.5                                                                               0.34                                ______________________________________                                    

                  TABLE 9                                                          ______________________________________                                         1000:1 Wt. Ratio DMDMH/IPBC                                                    Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600    0.1    99.9                                                                               0.06                               0.01%   ECOLI    100      800    0.1    99.9                                                                               0.13                               0.01%   PSA      1200    1600    0.1    99.9                                                                               0.06                               0.01%   PC       1800    1600    0.1    99.9                                                                               0.06                               0.01%   CAN      100     16000   0.1    99.9                                                                               0.01                               0.01%   AN       100     16000   0.1    99.9                                                                               0.01                                0.025% SA       200     1600    0.25                                                                                 249.8                                                                               0.16                                0.025% ECOLI    100      800    0.25                                                                                 249.8                                                                               0.31                                0.025% PSA      1200    1600    0.25                                                                                 249.8                                                                               0.16                                0.025% PC       1800    1600    0.25                                                                                 249.8                                                                               0.16                                0.025% CAN      100     16000   0.25                                                                                 249.8                                                                               0.02                                0.025% AN       100     16000   0.25                                                                                 249.8                                                                               0.02                               0.05%   SA       200     1600    0.5   499.5                                                                               0.31                               0.05%   ECOLI    100      800    0.5   499.5                                                                               0.63                               0.05%   PSA      1200    1600    0.5   499.5                                                                               0.31                               0.05%   PC       1800    1600    0.5   499.5                                                                               0.31                               0.05%   CAN      100     16000   0.5   499.5                                                                               0.04                               0.05%   AN       100     16000   0.5   499.5                                                                               0.04                               0.10%   SA       200     1600  1      999   0.63                               0.10%   ECOLI    100      800  1      999   1.26                               0.10%   PSA      1200    1600  1      999   0.63                               0.10%   PC       1800    1600  1      999   0.62                               0.10%   CAN      100     16000 1      999   0.07                               0.10%   AN       100     16000 1      999   0.07                               0.20%   SA       200     1600  2     1998   1.26                               0.20%   ECOLI    100      800  2     1998   2.52                               0.20%   PSA      1200    1600  2     1998   1.25                               0.20%   PC       1800    1600  2     1998   1.25                               0.20%   CAN      100     16000 2     1998   0.14                               0.20%   AN       100     16000 2     1998   0.14                               0.40%   SA       200     1600  4     3996   2.52                               0.40%   ECOLI    100      800  4     3996   5.04                               0.40%   PSA      1200    1600  4     3996   2.50                               0.40%   PC       1800    1600  4     3996   2.50                               0.40%   CAN      100     16000 4     3996   0.29                               0.40%   AN       100     16000 4     3996   0.29                               0.50%   SA       200     1600  5     4995   3.15                               0.50%   ECOLI    100      800  5     4995   6.29                               0.50%   PSA      1200    1600  5     4995   3.13                               0.50%   PC       1800    1600  5     4995   3.12                               0.50%   CAN      100     16000 5     4995   0.36                               0.50%   AN       100     16000   2.5   4997.5                                                                              0.36                               ______________________________________                                    

                  TABLE 10                                                         ______________________________________                                         500:1 Wt. Ratio DMDMH/IPBC                                                     Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                             Q.sub.B                                                                               SI                                  ______________________________________                                         0.01%   SA       200     1600    0.2                                                                                  99.8                                                                               0.06                                0.01%   ECOLI    100      800    0.2                                                                                  99.8                                                                               0.13                                0.01%   PSA      1200    1600    0.2                                                                                  99.8                                                                               0.06                                0.01%   PC       1800    1600    0.2                                                                                  99.8                                                                               0.06                                0.01%   CAN      100     16000   0.2                                                                                  99.8                                                                               0.01                                0.01%   AN       100     16000   0.2                                                                                  99.8                                                                               0.01                                 0.25%  SA       200     1600    0.5                                                                                 249.5                                                                               0.16                                 0.25%  ECOLI    100      800    0.5                                                                                 249.5                                                                               0.32                                 0.25%  PSA      1200    1600    0.5                                                                                 249.5                                                                               0.16                                 0.25%  PC       1800    1600    0.5                                                                                 249.5                                                                               0.16                                 0.25%  CAN      100     16000   0.5                                                                                 249.5                                                                               0.02                                 0.25%  AN       100     16000   0.5                                                                                 249.5                                                                               0.02                                0.05%   SA       200     1600  1     499   0.32                                0.05%   ECOLI    100      800  1     499   0.63                                0.05%   PSA      1200    1600  1     499   0.31                                0.05%   PC       1800    1600  1     499   0.31                                0.05%   CAN      100     16000 1     499   0.04                                0.05%   AN       100     16000 1     499   0.04                                0.10%   SA       200     1600  2     998   0.63                                0.10%   ECOLI    100      800  2     998   1.27                                0.10%   PSA      1200    1600  2     998   0.63                                0.10%   PC       1800    1600  2     998   0.62                                0.10%   CAN      100     16000 2     998   0.08                                0.10%   AN       100     16000 2     998   0.08                                0.20%   SA       200     1600  4    1996   1.27                                0.20%   ECOLI    100      800  4    1996   2.54                                0.20%   PSA      1200    1600  4    1996   1.25                                0.20%   PC       1800    1600  4    1996   1.25                                0.20%   CAN      100     16000 4    1996   0.16                                0.20%   AN       100     16000 4    1996   0.16                                0.40%   SA       200     1600  8    3992   2.54                                0.40%   ECOLI    100      800  8    3992   5.07                                0.40%   PSA      1200    1600  8    3992   2.50                                0.40%   PC       1800    1600  8    3992   2.50                                0.40%   CAN      100     16000 8    3992   0.33                                0.40%   AN       100     16000 8    3992   0.33                                0.50%   SA       200     1600  10   4900   3.11                                0.50%   ECOLI    100      800  10   4900   6.23                                0.50%   PSA      1200    1600  10   4900   3.07                                0.50%   PC       1800    1600  10   4900   3.07                                0.50%   CAN      100     16000 10   4900   0.41                                0.50%   AN       100     16000 10   4900   0.41                                ______________________________________                                    

                  TABLE 11                                                         ______________________________________                                         200:1 Wt. Ratio DMDMH/IPBC                                                     Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                               Q.sub.B                                                                              SI                                 ______________________________________                                         0.01%   SA       200     1600    0.5   99.5 0.06                               0.01%   ECOLI    100      800    0.5   99.5 0.13                               0.01%   PSA      1200    1600    0.5   99.5 0.06                               0.01%   PC       1800    1600    0.5   99.5 0.06                               0.01%   CAN      100     16000   0.5   99.5 0.01                               0.01%   AN       100     16000   0.5   99.5 0.01                                0.025% SA       200     1600     1.25                                                                                248.75                                                                              0.16                                0.025% ECOLI    100      800     1.25                                                                                248.75                                                                              0.32                                0.025% PSA      1200    1600     1.25                                                                                248.75                                                                              0.16                                0.025% PC       1800    1600     1.25                                                                                248.75                                                                              0.16                                0.025% CAN      100     16000    1.25                                                                                248.75                                                                              0.03                                0.025% AN       100     16000    1.25                                                                                248.75                                                                              0.03                               0.05%   SA       200     1600    2.5  497.5 0.32                               0.05%   ECOLI    100      800    2.5  497.5 0.65                               0.05%   PSA      1200    1600    2.5  497.5 0.31                               0.05%   PC       1800    1600    2.5  497.5 0.31                               0.05%   CAN      100     16000   2.5  497.5 0.06                               0.05%   AN       100     16000   2.5  497.5 0.06                               0.10%   SA       200     1600   5     995   0.65                               0.10%   ECOLI    100      800   5     995   1.29                               0.10%   PSA      1200    1600   5     995   0.63                               0.10%   PC       1800    1600   5     995   0.62                               0.10%   CAN      100     16000  5     995   0.11                               0.10%   AN       100     16000  5     995   0.11                               0.20%   SA       200     1600  10     1990  1.29                               0.20%   ECOLI    100      800  10     1990  2.59                               0.20%   PSA      1200    1600  10     1990  1.25                               0.20%   PC       1800    1600  10     1990  1.25                               0.20%   CAN      100     16000 10     1990  0.22                               0.20%   AN       100     16000 10     1990  0.22                               0.40%   SA       200     1600  20     3980  2.59                               0.40%   ECOLI    100      800  20     3980  5.18                               0.40%   PSA      1200    1600  20     3980  2.50                               0.40%   PC       1800    1600  20     3980  2.50                               0.40%   CAN      100     16000 20     3980  0.45                               0.40%   AN       100     16000 20     3980  0.45                               0.50%   SA       200     1600  25     4975  3.23                               0.50%   ECOLI    100      800  25     4975  6.47                               0.50%   PSA      1200    1600  25     4975  3.13                               0.50%   PC       1800    1600  25     4975  3.12                               0.50%   CAN      100     16000 25     4975  0.56                               0.50%   AN       100     16000 25     4975  0.56                               ______________________________________                                    

                  TABLE 12                                                         ______________________________________                                         100:1 Wt. Ratio DMDMH/IPBC                                                     Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                              SI                                  ______________________________________                                         0.01%   SA       200     1600   1     99   0.07                                0.01%   ECOLI    100      800   1     99   0.13                                0.01%   PSA      1200    1600   1     99   0.06                                0.01%   PC       1800    1600   1     99   0.06                                0.01%   CAN      100     16000  1     99   0.02                                0.01%   AN       100     16000  1     99   0.02                                 0.025% SA       200     1600    2.5 248   0.17                                 0.025% ECOLI    100      800    2.5 248   0.33                                 0.025% PSA      1200    1600    2.5 248   0.16                                 0.025% PC       1800    1600    2.5 248   0.16                                 0.025% CAN      100     16000   2.5 248   0.04                                 0.025% AN       100     16000   2.5 248   0.04                                0.05%   SA       200     1600   5    495   0.33                                0.05%   ECOLI    100      800   5    495   0.67                                0.05%   PSA      1200    1600   5    495   0.31                                0.05%   PC       1800    1600   5    495   0.31                                0.05%   CAN      100     16000  5    495   0.08                                0.05%   AN       100     16000  5    495   0.08                                0.10%   SA       200     1600  10    990   0.67                                0.10%   ECOLI    100      800  10    990   1.34                                0.10%   PSA      1200    1600  10    990   0.63                                0.10%   PC       1800    1600  10    990   0.62                                0.10%   CAN      100     16000 10    990   0.16                                0.10%   AN       100     16000 10    990   0.16                                0.20%   SA       200     1600  20    1980  1.34                                0.20%   ECOLI    100      800  20    1980  2.68                                0.20%   PSA      1200    1600  20    1980  1.25                                0.20%   PC       1800    1600  20    1980  1.25                                0.20%   CAN      100     16000 20    1980  0.32                                0.20%   AN       100     16000 20    1980  0.32                                0.40%   SA       200     1600  40    3960  2.68                                0.40%   ECOLI    100      800  40    3960  5.35                                0.40%   PSA      1200    1600  40    3960  2.51                                0.40%   PC       1800    1600  40    3960  2.50                                0.40%   CAN      100     16000 40    3960  0.65                                0.40%   AN       100     16000 40    3960  0.65                                0.50%   SA       200     1600  50    4950  3.34                                0.50%   ECOLI    100      800  50    4950  6.69                                0.50%   PSA      1200    1600  50    4950  3.14                                0.50%   PC       1800    1600  50    4950  3.12                                0.50%   CAN      100     16000 50    4950  0.81                                0.50%   AN       100     16000 50    4950  0.81                                ______________________________________                                    

                  TABLE 13                                                         ______________________________________                                         50:1 Wt. Ratio DMDMH/IPBC                                                      Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                              SI                                  ______________________________________                                         0.01%   SA       200     1600   2     98   0.07                                0.01%   ECOLI    100      800   2     98   0.14                                0.01%   PSA      1200    1600   2     98   0.06                                0.01%   PC       1800    1600   2     98   0.06                                0.01%   CAN      100     16000  2     98   0.03                                0.01%   AN       100     16000  2     98   0.03                                 0.025% SA       200     1600   5    245   0.18                                 0.025% ECOLI    100      800   5    245   0.36                                 0.025% PSA      1200    1600   5    245   0.16                                 0.025% PC       1800    1600   5    245   0.16                                 0.025% CAN      100     16000  5    245   0.07                                 0.025% AN       100     16000  5    245   0.07                                0.05%   SA       200     1600  10    490   0.36                                0.05%   ECOLI    100      800  10    490   0.71                                0.05%   PSA      1200    1600  10    490   0.31                                0.05%   PC       1800    1600  10    490   0.31                                0.05%   CAN      100     16000 10    490   0.13                                0.05%   AN       100     16000 10    490   0.13                                0.10%   SA       200     1600  20    980   0.71                                0.10%   ECOLI    100      800  20    980   1.43                                0.10%   PSA      1200    1600  20    980   0.63                                0.10%   PC       1800    1600  20    980   0.62                                0.10%   CAN      100     16000 20    980   0.26                                0.10%   AN       100     16000 20    980   0.26                                0.20%   SA       200     1600  40    1960  1.43                                0.20%   ECOLI    100      800  40    1960  2.85                                0.20%   PSA      1200    1600  40    1960  1.26                                0.20%   PC       1800    1600  40    1960  1.25                                0.20%   CAN      100     16000 40    1960  0.52                                0.20%   AN       100     16000 40    1960  0.52                                0.40%   SA       200     1600  80    3920  2.85                                0.40%   ECOLI    100      800  80    3920  5.70                                0.40%   PSA      1200    1600  80    3920  2.52                                0.40%   PC       1800    1600  80    3920  2.49                                0.40%   CAN      100     16000 80    3920  1.05                                0.40%   AN       100     16000 80    3920  1.05                                0.50%   SA       200     1600  100   4900  3.56                                0.50%   ECOLI    100      800  100   4900  7.13                                0.50%   PSA      1200    1600  100   4900  3.15                                0.50%   PC       1800    1600  100   4900  3.12                                0.50%   CAN      100     16000 100   4900  1.31                                0.50%   AN       100     16000 100   4900  1.31                                ______________________________________                                    

                  TABLE 14                                                         ______________________________________                                         20:1 Wt. Ratio DMDMH/IPBC                                                      Use Level                                                                              Organism Q.sub.a Q.sub.b                                                                              Q.sub.A                                                                              Q.sub.B                                                                               SI                                 ______________________________________                                         0.01%   SA       200     1600   5     95    0.08                               0.01%   ECOLI    100      800   5     95    0.17                               0.01%   PSA      1200    1600   5     95    0.06                               0.01%   PC       1800    1600   5     95    0.06                               0.01%   CAN      100     16000  5     95    0.06                               0.01%   AN       100     16000  5     95    0.06                                0.025% SA       200     1600    12.5                                                                                 237.5                                                                               0.21                                0.025% ECOLI    100      800    12.5                                                                                 237.5                                                                               0.42                                0.025% PSA      1200    1600    12.5                                                                                 237.5                                                                               0.16                                0.025% PC       1800    1600    12.5                                                                                 237.5                                                                               0.16                                0.025% CAN      100     16000   12.5                                                                                 237.5                                                                               0.14                                0.025% AN       100     16000   12.5                                                                                 237.5                                                                               0.14                               0.05%   SA       200     1600   25    475   0.42                               0.05%   ECOLI    100      800   25    475   0.84                               0.05%   PSA      1200    1600   25    475   0.32                               0.05%   PC       1800    1600   25    475   0.31                               0.05%   CAN      100     16000  25    475   0.28                               0.05%   AN       100     16000  25    475   0.28                               0.10%   SA       200     1600   50    950   0.84                               0.10%   ECOLI    100      800   50    950   1.69                               0.10%   PSA      1200    1600   50    950   0.64                               0.10%   PC       1800    1600   50    950   0.62                               0.10%   CAN      100     16000  50    950   0.56                               0.10%   AN       100     16000  50    950   0.56                               0.20%   SA       200     1600  100   1900   1.69                               0.20%   ECOLI    100      800  100   1900   3.38                               0.20%   PSA      1200    1600  100   1900   1.27                               0.20%   PC       1800    1600  100   1900   1.24                               0.20%   CAN      100     16000 100   1900   1.12                               0.20%   AN       100     16000 100   1900   1.12                               0.40%   SA       200     1600  200   4800   4.00                               0.40%   ECOLI    100      800  200   4800   8.00                               0.40%   PSA      1200    1600  200   4800   3.17                               0.40%   PC       1800    1600  200   4800   3.11                               0.40%   CAN      100     16000 200   4800   2.30                               0.40%   AN       100     16000 200   4800   2.30                               0.50%   SA       200     1600  250   4750   4.22                               0.50%   ECOLI    100      800  250   4750   8.44                               0.50%   PSA      1200    1600  250   4750   3.18                               0.50%   PC       1800    1600  250   4750   3.11                               0.50%   CAN      100     16000 250   4750   2.80                               0.50%   AN       100     16000 250   4750   2.80                               ______________________________________                                    

Similar SI results also were found with GADM and SUTTOCIDE® A as the methylol compound in place of Germall® II or DMDMH in admixtures with IPBC over the same wt. ratios and use level ranges as shown in the Tables 1-14 above.

Tables 1 through 14 above illustrate the synergism of IPBC (compound B) with Germall® II or DMDMH (compound A) at weight ratios of A:B of 2000:1, 1000:1, 500:1, 200:1, 100:1, 50:1 and 20:1. Synergism is very effective for all ratios at low use levels, e.g. 0.01% to 0.1%, against all tested gram-positive, gram-negative organisms and fungi organisms. At slightly higher use concentrations, e.g. 0.20 to 0.50%, all tested ratios were synergistic against Candida albicans and A. niger also. However, at 50:1 and 20:1 ratios, the synergistic effect is negligible at the 0.01 to 0.1% use levels, and non-synergistic even against Candida albicans and A. niger at use levels of 0.20 to 0.50%.

The SI values were lower for Germall® II as the methylol compound in the admixtures as compared to DMDMH.

Similar results were obtained when iodopropynyl alcohol (IPGA) was substituted for IPBC in the admixtures described above.

3. PRESERVATIVE ACTIVITY (CHALLENGE TEST)

A typical cosmetic emulsion was prepared for microbiological Challenge testing and predetermined admixtures of a methylol compound and IPBC were added at various use levels. The emulsion thus prepared had the following composition:

    ______________________________________                                                             % wt.                                                      ______________________________________                                         Phase A                                                                        Stearic Acid          5.00                                                     Mineral Oil           2.50                                                     Cetyl Alcohol         1.00                                                     Lareth-5 and Ceteth-5 and                                                                            0.50                                                     Oleth-5 and Steareth-5                                                         Glycerol Monostearate and                                                                            1.50                                                     Polyoxyethylene Stearate                                                       Phase B                                                                        Deionized Water       88.0                                                     Triethanolamine 99%   1.00                                                     Citric Acid 30% aqueous solution                                                                     0.60                                                     Preservative Admixture                                                                               qs                                                       ______________________________________                                    

To prepare the emulsion, Phases A and B were heated separately to 75°-80° C. Phase A then was added to Phase B with mixing. The mixture then was cooled to 55°-60° C. At this point the desired amount of the preservative admixture was added and the product was cooled to 50° C. while stirring. The citric acid solution then was added to adjust the pH and the mixture was stirred until a temperature of 30° C. was reached.

The challenge tests were carried out using the following microorganisms: SA, ECOLI, PSA, PC, AN and CAN, in this manner. 50 g. aliquots of the test emulsion containing various amounts of the preservative admixture were inoculated with approximately 10⁷ -10⁸ of the challenge organisms. The test samples then were stirred to disperse the challenge inoculum. The samples were incubated and assayed at 48 hours, 7, 14, 21 and 28 days. The assays were performed on 1 g. of the test sample by serially diluting 10¹ to 10⁶ of the original concentration. The plating medium for bacteria was Letheen agar and for fungi it was low pH Mycophil agar with Tween 20. Each plated sample was incubated for 48 hours at 37° C. for bacteria, 5 days at 25° C. for mold, and 3 days at 25° C. for fungi. After incubation, readings of the number of colonies per milliliter (cfu/ml) were made. At 21 days the test product was reinoculated with half of the original inoculum. The data is presented in Tables 15-23 below.

                                      TABLE 15                                     __________________________________________________________________________     2000:1 GERMALL ® II/IPBC                                                   __________________________________________________________________________     Test Level                                                                           Organism                                                                             48 Hours                                                                            7 Days                                                                              14 Days                                                                             21 Days                                                                              28 Days                                       __________________________________________________________________________     0.01% AN    69,000                                                                              260,000                                                                             190,000                                                                             17,000                                                                               4,500                                         0.01% CAN   98,000                                                                              76,000                                                                              1,400                                                                               3,100 19,000                                        0.01% ECOLI 110,000                                                                             290,000                                                                             2,400                                                                               138,000                                                                              560,000                                       0.01% PC    <10  <10  <10  <10   <10                                           0.01% PSA   <10  <10  <10  <10   <10                                           0.01% SA    190,000                                                                             220  <10  <10   3,700                                          0.025%                                                                              AN    2,800                                                                               10   10   <10   220                                            0.025%                                                                              CAN   58,000                                                                              29,000                                                                              18,000                                                                              56,000                                                                               110,000                                        0.025%                                                                              ECOLI 39,000                                                                              10   <10  <10   <10                                            0.025%                                                                              PC    <10  <10  <10  <10   <10                                            0.025%                                                                              PSA   <10  <10  <10  <10   <10                                            0.025%                                                                              SA    37,000                                                                              170  <10  <10   <10                                           0.05% AN    20   <10  <10  <10   <10                                           0.05% CAN   19,000                                                                              6,600                                                                               70   <10   320                                           0.05% ECOLI 3,400                                                                               <10  <10  <10   <10                                           0.05% PC    <10  <10  <10  <10   <10                                           0.05% PSA   <10  <10  <10  <10   <10                                           0.05% SA    31,000                                                                              <10  <10  <10   <10                                           0.1%  AN    <10  <10  <10  <10   <10                                           0.1%  CAN   180  <10  <10  <10   <10                                           0.1%  ECOLI <10  <10  <10  <10   <10                                           0.1%  PC    <10  <10  <10  <10   <10                                           0.1%  PSA   <10  <10  <10  <10   <10                                           0.1%  SA    750  <10  <10  <10   <10                                           0.2%  AN    <10  <10  <10  <10   <10                                           0.2%  CAN   <10  <10  <10  <10   <10                                           0.2%  ECOLI <10  <10  <10  <10   <10                                           0.2%  PC    <10  <10  <10  <10   <10                                           0.2%  PSA   <10  <10  <10  <10   <10                                           0.2%  SA    <10  <10  <10  <10   <10                                           Unpreserved control                                                            AN          52,000                                                                              27,000                                                                              19,000                                                                              19,000                                                                               19,000                                        CAN         110,000                                                                             130,000                                                                             240,000                                                                             180,000                                                                              240,000                                       ECOLI       54,000                                                                              140,000                                                                             170,000                                                                             170,000                                                                              74,000                                        PC          6,400,000                                                                           6,400,000                                                                           2,000,000                                                                           6,700,000                                                                            29,000                                        PSA         110,000                                                                             700  110,000                                                                             290,000                                                                              85,000                                        SA          2,800,000                                                                           250,000                                                                             51,000                                                                              3,700 330                                           Inoculum Concentration                                                                     0 Hours                                                                             21 Days                                                       AN          26,000                                                                              53,000                                                        CAN         1,000,000                                                                           1,900,000                                                     ECOLI       3,600,000                                                                           170,000                                                       PC          3,400,000                                                                           87,000                                                        PSA         4,500,000                                                                           390,000                                                       SA          4,100,000                                                                           200,000                                                       __________________________________________________________________________

                                      TABLE 16                                     __________________________________________________________________________     1000:1 GERMALL ® II/IPBC                                                   __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                              14 Days                                                                              21 Days                                                                             28 Days                                       __________________________________________________________________________     0.01% AN   34,000                                                                               3,500                                                                               80    10   <10                                           0.01% CAN  420,000                                                                              24,000                                                                              950   6,400                                                                               6,400,000                                     0.01% ECOLI                                                                               120,000                                                                              63,000                                                                              93,000                                                                               92,000                                                                              9,600,000                                     0.01% PC   10    25,000                                                                              1,600 15,800                                                                              33,000,000                                    0.01% PSA  <10   <10  <10   <10  <10                                           0.01% SA   100,000                                                                              1,400                                                                               <10   <10  5,000                                          0.025%                                                                              AN   530   10   <10   <10  <10                                            0.025%                                                                              CAN  34,000                                                                               750  10    770  240,000                                        0.025%                                                                              ECOLI                                                                               120,000                                                                              <10  <10   <10  <10                                            0.025%                                                                              PC   <10   <10  <10   <10  <10                                            0.025%                                                                              PSA  <10   <10  <10   <10  <10                                            0.025%                                                                              SA   37,000                                                                               170  <10   <10  <10                                           0.05% AN   <10   <10  <10   <10  <10                                           0.05% CAN  13,000                                                                               <10  <10   <10  <10                                           0.05% ECOLI                                                                               68,000                                                                               <10  <10   <10  <10                                           0.05% PC   <10   <10  <10   <10  <10                                           0.05% PSA  <10   < 10 <10   <10  <10                                           0.05% SA   21,000                                                                               <10  <10   <10  <10                                           0.1%  AN   <10   <10  <10   <10  <10                                           0.1%  CAN  10    <10  <10   <10  <10                                           0.1%  ECOLI                                                                               <10   <10  <10   <10  <10                                           0.1%  PC   <10   <10  <10   <10  <10                                           0.1%  PSA  <10   <10  <10   <10  <10                                           0.1%  SA   1,400 <10  <10   <10  <10                                           0.2%  AN   <10   <10  <10   <10  <10                                           0.2%  CAN  <10   <10  <10   <10  <10                                           0.2%  ECOLI                                                                               <10   <10  <10   <10  <10                                           0.2%  PC   <10   <10  <10   <10  <10                                           0.2%  PSA  <10   <10  <10   <10  <10                                           0.2%  SA   <10   <10  <10   <10  <10                                           Unpreserved control                                                            AN         52,000                                                                               27,000                                                                              19,000                                                                               19,000                                                                              19,000                                        CAN        110,000                                                                              130,000                                                                             240,000                                                                              180,000                                                                             240,000                                       ECOLI      54,000                                                                               140,000                                                                             170,000                                                                              170,000                                                                             74,000                                        PC         6,400,000                                                                            6,400,000                                                                           2,000,000                                                                            6,700,000                                                                           29,000                                        PSA        110,000                                                                              700  110,000                                                                              290,000                                                                             85,000                                        SA         2,800,000                                                                            250,000                                                                             51,000                                                                               3,700                                                                               330                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         26,000                                                                               53,000                                                        CAN        1,000,000                                                                            1,900,000                                                     ECOLI      3,600,000                                                                            170,000                                                       PC         3,400,000                                                                            87,000                                                        PSA        4,500,000                                                                            390,000                                                       SA         4,100,000                                                                            200,000                                                       __________________________________________________________________________

                                      TABLE 17                                     __________________________________________________________________________     500:1 GERMALL ® II/IPBC                                                    __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                               14 Days                                                                             21 Days                                                                             28 Days                                       __________________________________________________________________________     0.01% AN   23,000                                                                               40    <10  <10  <10                                           0.01% CAN  170,000                                                                              5,600 290  200  <10                                           0.01% ECOLI                                                                               90,000                                                                               57,000                                                                               95,000                                                                              70,000                                                                              240,000                                       0.01% PC   10    <10   <10  >10,000                                                                             42,000,000                                    0.01% PSA  <10   <10   <10  <10  <10                                           0.01% SA   380,000                                                                              440   <10  <10  5,100                                         0.05% AN   <10   <10   <10  <10  <10                                           0.05% CAN  8,700 <10   <10  <10  <10                                           0.05% ECOLI                                                                               60,000                                                                               <10   <10  <10  <10                                           0.05% PC   <10   <10   <10  <10  <10                                           0.05% PSA  <10   <10   <10  <10  <10                                           0.05% SA   31,000                                                                               <10   <10  <10  <10                                           0.1%  AN   <10   <10   <10  <10  <10                                           0.1%  CAN  <10   <10   <10  <10  <10                                           0.1%  ECOLI                                                                               <10   <10   <10  <10  <10                                           0.1%  PC   <10   <10   <10  <10  <10                                           0.1%  PSA  <10   <10   <10  <10  <10                                           0.1%  SA   890   <10   <10  <10  <10                                           0.2%  AN   <10   <10   <10  <10  <10                                           0.2%  CAN  <10   <10   <10  <10  <10                                           0.2%  ECOLI                                                                               <10   <10   <10  <10  <10                                           0.2%  PC   <10   <10   <10  <10  <10                                           0.2%  PSA  <10   <10   <10  <10  <10                                           0.2%  SA   <10   <10   <10  <10  <10                                           Unpreserved control                                                            AN         6,100 520,000                                                                              18,000                                                                              5,000                                                                               11,000                                        CAN        1,000,000                                                                            710,000                                                                              95,000                                                                              12,000                                                                              64,000                                        ECOLI      7,100,000                                                                            6,200,000                                                                            610,000                                                                             350,000                                                                             120,000                                       PC         14,600,000                                                                           160,000,000                                                                          3,600,000                                                                           2,720,000                                                                           9,500,000                                     PSA        20    900   130  4,100                                                                               >100,000                                      SA         43,000,000                                                                           600,000                                                                              1,000                                                                               220  <10                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         19,000                                                                               4,700,000                                                     CAN        340,000                                                                              16,000,000                                                    ECOLI      3,900,000                                                                            1,480,000                                                     PC         3,800,000                                                                            1,380,000                                                     PSA        9,200,000                                                                            730,000                                                       SA         4,800,000                                                                            360,000                                                       __________________________________________________________________________

                                      TABLE 18                                     __________________________________________________________________________     200:1 GERMALL ® II/IPBC                                                    __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                              14 Days                                                                              21 Days                                                                             28 Days                                       __________________________________________________________________________     0.01% AN   47,000                                                                               320  10    <10  <10                                           0.01% CAN  810,000                                                                              450,000                                                                             410,000                                                                              190,000                                                                             63,000                                        0.01% ECOLI                                                                               220,000                                                                              7,600                                                                               <10   850  >1,000,000                                    0.01% PC   10,000                                                                               500,000                                                                             1,900,000                                                                            1,100,000                                                                           193,000                                       0.01% PSA  <10   <10  <10   <10  <10                                           0.01% SA   190,000                                                                              23,000                                                                              120   <10  <10                                           0.05% AN   <10   <10  <10   <10  <10                                           0.05% CAN  190   <10  <10   <10  <10                                           0.05% ECOLI                                                                               37,000                                                                               <10  <10   <10  <10                                           0.05% PC   <10   <10  <10   <10  <10                                           0.05% PSA  <10   <10  <10   <10  <10                                           0.05% SA   19,000                                                                               <10  <10   <10  <10                                           0.1%  AN   <10   <10  <10   <10  <10                                           0.1%  CAN  10    <10  <10   <10  <10                                           0.1%  ECOLI                                                                               <10   <10  <10   < 10 <10                                           0.1%  PC   <10   <10  <10   <10  <10                                           0.1%  PSA  <10   <10  <10   <10  <10                                           0.1%  SA   45,000                                                                               <10  <10   <10  <10                                           0.2%  AN   <10   <10  <10   <10  <10                                           0.2%  CAN  <10   <10  <10   <10  <10                                           0.2%  ECOLI                                                                               <10   <10  <10   <10  <10                                           0.2%  PC   <10   <10  <10   <10  <10                                           0.2%  PSA  <10   <10  <10   <10  <10                                           0.2%  SA   <10   <10  <10   <10  <10                                           Unpreserved control                                                            AN         89,000                                                                               32,000                                                                              22,000                                                                               16,000                                                                              16,000                                        CAN        210,000                                                                              670,000                                                                             430,000                                                                              590,000                                                                             640,000                                       ECOLI      640,000                                                                              360,000                                                                             410,000                                                                              990,000                                                                             68,000                                        PC         19,000,000                                                                           3,200,000                                                                           7,000,000                                                                            >10,000                                                                             2,760,000                                     PSA        80    9,400                                                                               200,000                                                                              >10,000                                                                             34,000                                        SA         6,300,000                                                                            190,000                                                                             11,000                                                                               580  120                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         41,000                                                                               32,000                                                        CAN        640   1,100,000                                                     ECOLI      5,800,000                                                                            1,300,000                                                     PC         900,000                                                                              3,000,000                                                     PSA        1,800,000                                                                            4,900,000                                                     SA         7,200,000                                                                            2,000,000                                                     __________________________________________________________________________

                                      TABLE 19                                     __________________________________________________________________________     50:1 GERMALL ® II/IPBC                                                     __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                              14 Days                                                                              21 Days                                                                             28 Days                                       __________________________________________________________________________     0.01% AN   4,100 40   <10   <10  <10                                           0.01% CAN  310,000                                                                              7,700                                                                               560   5,600                                                                               5,200                                         0.01% ECOLI                                                                               170,000                                                                              710  10    <10  120                                           0.01% PC   7,400 74,000                                                                              340,000                                                                              720,000                                                                             520,000                                       0.01% PSA  <10   <10  <10   <10  30                                            0.01% SA   110,000                                                                              11,000                                                                              <10   <10  9,200                                         0.05% AN   <10   100  <10   <10  <10                                           0.05% CAN  210   <10  <10   <10  <10                                           0.05% ECOLI                                                                               150,000                                                                              <10  <10   <10  <10                                           0.05% PC   <10   <10  <10   <10  <10                                           0.05% PSA  <10   <10  <10   <10  <10                                           0.05% SA   35,000                                                                               <10  <10   <10  <10                                           0.1%  AN   <10   <10  <10   <10  <10                                           0.1%  CAN  <10   <10  <10   <10  <10                                           0.1%  ECOLI                                                                               510   <10  <10   <10  <10                                           0.1%  PC   <10   <10  <10   <10  <10                                           0.1%  PSA  <10   <10  <10   <10  <10                                           0.1%  SA   3,000 <10  <10   <10  <10                                           0.2%  AN   <10   <10  <10   <10  <10                                           0.2%  CAN  <10   <10  <10   <10  <10                                           0.2%  ECOLI                                                                               <10   <10  <10   <10  <10                                           0.2%  PC   <10   <10  <10   <10  <10                                           0.2%  PSA  <10   <10  <10   <10  <10                                           0.2%  SA   <10   <10  <10   <10  <10                                           Unpreserved control                                                            AN         89,000                                                                               32,000                                                                              22,000                                                                               16,000                                                                              16,000                                        CAN        210,000                                                                              670,000                                                                             430,000                                                                              590,000                                                                             640,000                                       ECOLI      640,000                                                                              360,000                                                                             410,000                                                                              990,000                                                                             68,000                                        PC         19,000,000                                                                           3,200,000                                                                           7,000,000                                                                            >10,000                                                                             2,760,000                                     PSA        80    9,400                                                                               200,000                                                                              >10,000                                                                             34,000                                        SA         6,300,000                                                                            190,000                                                                             11,000                                                                               580  120                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         41,000                                                                               32,000                                                        CAN        640   1,100,000                                                     ECOLI      5,800,000                                                                            1,300,000                                                     PC         900,000                                                                              3,000,000                                                     PSA        1,800,000                                                                            4,900,000                                                     SA         7,200,000                                                                            2,000,000                                                     __________________________________________________________________________

                                      TABLE 20                                     __________________________________________________________________________     20:1 GERMALL ® II/IPBC                                                     __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                              14 Days                                                                             21 Days                                                                              28 Days                                       __________________________________________________________________________     0.01% AN   3,100 <10  <10  <10   <10                                           0.01% CAN  75,000                                                                               220  <10  <10   2,400                                         0.01% ECOLI                                                                               160,000                                                                              110  <10  <10   20                                            0.01% PC   12,000                                                                               1,000,000                                                                           2,100,000                                                                           >1,000,000                                                                           730,000                                       0.01% PSA  <10   <10  <10  <10   4,000                                         0.01% SA   140,000                                                                              4,100                                                                               <10  <10   1,680                                         0.05% AN   <10   <10  <10  <10   <10                                           0.05% CAN  <10   <10  <10  <10   <10                                           0.05% ECOLI                                                                               16,000                                                                               <10  <10  <10   <10                                           0.05% PC   <10   <10  <10  <10   <10                                           0.05% PSA  <10   <10       <10   <10                                           0.05% SA   31,000                                                                               <10  <10  <10   <10                                           0.1%  AN   <10   <10  <10  <10   <10                                           0.1%  CAN  <10   <10  <10  <10   <10                                           0.1%  ECOLI                                                                               <10   <10  <10  <10   <10                                           0.1%  PC   < 10  <10  <10  <10   <10                                           0.1%  PSA  <10   <10  <10  <10   <10                                           0.1%  SA   6,800 <10  <10  <10   <10                                           0.2%  AN   <10   <10  <10  <10   <10                                           0.2%  CAN  <10   <10  <10  <10   <10                                           0.2%  ECOLI                                                                               <10   <10  <10  <10   <10                                           0.2%  PC   <10   <10  <10  <10   <10                                           0.2%  PSA  <10   <10  <10  <10   <10                                           0.2%  SA   <10   <10  <10  <10   <10                                           Unpreserved control                                                            AN         89,000                                                                               32,000                                                                              22,000                                                                              16,000                                                                               16,000                                        CAN        210,000                                                                              670,000                                                                             430,000                                                                             590,000                                                                              640,000                                       ECOLI      640,000                                                                              360,000                                                                             410,000                                                                             990,000                                                                              68,000                                        PC         19,000,000                                                                           3,200,000                                                                           7,000,000                                                                           >10,000                                                                              2,760,000                                     PSA        80    9,400                                                                               200,000                                                                             >10,000                                                                              34,000                                        SA         6,300,000                                                                            190,000                                                                             11,000                                                                              580   120                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         41,000                                                                               32,000                                                        CAN        640   1,100,000                                                     ECOLI      5,800,000                                                                            1,300,000                                                     PC         900,000                                                                              3,000,000                                                     PSA        1,800,000                                                                            4,900,000                                                     SA         7,200,000                                                                            2,000,000                                                     __________________________________________________________________________

                                      TABLE 21                                     __________________________________________________________________________     2000:1 DMDMH/IPBC                                                              __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                               14 Days                                                                             21 Days                                                                             28 Days                                       __________________________________________________________________________      0.025%                                                                              AN   4,100 38,000                                                                               270  80   100                                            0.025%                                                                              CAN  270,000                                                                              1,900,000                                                                            550,000                                                                             220,000                                                                             210,000                                        0.025%                                                                              ECOLI                                                                               1,300,000                                                                            <10   <10  <10  3,000                                          0.025%                                                                              PC   <10   <10   <10  <10  <10                                            0.025%                                                                              PSA  <10   <10   <10  <10  <10                                            0.025%                                                                              SA   42,000                                                                               20    <10  <10  <10                                           0.05% AN   <10   <10   <10  <10  <10                                           0.05% CAN  770,000                                                                              130,000                                                                              670,000                                                                             160,000                                                                             64,000                                        0.05% ECOLI                                                                               220,000                                                                              <10   <10  <10  <10                                           0.05% PC   <10   <10   <10  <10  <10                                           0.05% PSA  <10   <10   <10  <10  <10                                           0.05% SA   9,000 <10   <10  <10  <10                                           0.1%  AN   <10   <10   <10  <10  <10                                           0.1%  CAN  580   840   500  40,000                                                                              83,000                                        0.1%  ECOLI                                                                               340   <10   <10  <10  <10                                           0.1%  PC   <10   <10   <10  < 10 <10                                           0.1%  PSA  <10   <10   <10  <10  <10                                           0.1%  SA   29,000                                                                               <10   <10  <10  <10                                           0.2%  AN   <10   <10   <10  <10  <10                                           0.2%  CAN  <10   10    10   <10  21                                            0.2%  ECOLI                                                                               <10   <10   <10  <10  <10                                           0.2%  PC   <10   <10   <10  <10  <10                                           0.2%  PSA  <10   <10   <10  <10  <10                                           0.2%  SA   <10   <10   <10  <10  <10                                           Unpreserved control                                                            AN         37,000                                                                               36,000                                                                               24,000                                                                              5,200                                                                               6,000                                         CAN        120,000                                                                              1,900,000                                                                            3,300,000                                                                           480,000                                                                             790,000                                       ECOLI      150,000                                                                              2,500,000                                                                            7,300,000                                                                           240,000                                                                             140,000                                       PC         19,000,000                                                                           15,600,000                                                                           5,900,000                                                                           8,500,000                                                                           31,000,000                                    PSA        <10   <10   100  15,200                                                                              300,000                                       SA         7,000,000                                                                            >1,000,000                                                                           12,000                                                                              3,000                                                                               110                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         50,000                                                                               41,000                                                        CAN        1,400,000                                                                            640                                                           ECOLI      4,800,000                                                                            5,800,000                                                     PC         9,200,000                                                                            900,000                                                       PSA        6,900,000                                                                            9,000,000                                                     SA         5,700,000                                                                            7,200,000                                                     __________________________________________________________________________

                                      TABLE 22                                     __________________________________________________________________________     1000:1 DMDMH/IPBC                                                              __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                               14 Days                                                                             21 Days                                                                             28 Days                                       __________________________________________________________________________      0.025%                                                                              AN   650   900   <10  <10  140                                            0.025%                                                                              CAN  97,000                                                                               900,000                                                                              2,300,000                                                                           120,000                                                                             120,000                                        0.025%                                                                              ECOLI                                                                               160,000                                                                              <10   <10  <10  2,400                                          0.025%                                                                              PC   <10   <10   <10  <10  <10                                            0.025%                                                                              PSA  <10   <10   <10  <10  <10                                            0.025%                                                                              SA   23,000                                                                               <10   <10  <10  90                                            0.05% AN   20    <10   <10  <10  <10                                           0.05% CAN  65,000                                                                               520,000                                                                              56,000                                                                              32,000                                                                              370,000                                       0.05% ECOLI                                                                               26,000                                                                               <10   <10  <10  <10                                           0.05% PC   <10   <10   <10  <10  <10                                           0.05% PSA  <10   <10   <10  <10  <10                                           0.05% SA   12,000                                                                               <10   <10  <10  <10                                           0.1%  AN   <10   <10   <10  <10  <10                                           0.1%  CAN  3,100 4,800 180  640  4,400                                         0.1%  ECOLI                                                                               45,000                                                                               <10   <10  < 10 <10                                           0.1%  PC   <10   <10   <10  <10  <10                                           0.1%  PSA  <10   <10   <10  <10  <10                                           0.1%  SA   6,000 <10   <10  <10  <10                                           0.2%  AN   <10   <10   <10  <10  <10                                           0.2%  CAN  <10   <10   <10  <10  <10                                           0.2%  ECOLI                                                                               <10   <10   <10  <10  <10                                           0.2%  PC   <10   <10   <10  <10  <10                                           0.2%  PSA  <10   <10   <10  <10  <10                                           0.2%  SA   180   <10   <10  <10  <10                                           Unpreserved control                                                            AN         37,000                                                                               36,000                                                                               24,000                                                                              5,200                                                                               6,000                                         CAN        120,000                                                                              1,900,000                                                                            3,300,000                                                                           480,000                                                                             790,000                                       ECOLI      150,000                                                                              2,500,000                                                                            7,300,000                                                                           240,000                                                                             140,000                                       PC         19,000,000                                                                           15,600,000                                                                           5,900,000                                                                           8,500,000                                                                           31,000,000                                    PSA        <10   <10   100  15,200                                                                              300,000                                       SA         7,000,000                                                                            >1,000,000                                                                           12,000                                                                              3,000                                                                               110                                           Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         50,000                                                                               41,000                                                        CAN        1,400,000                                                                            640                                                           ECOLI      4,800,000                                                                            5,800,000                                                     PC         9,200,000                                                                            900,000                                                       PSA        6,900,000                                                                            9,000,000                                                     SA         5,700,000                                                                            7,200,000                                                     __________________________________________________________________________

                                      TABLE 23                                     __________________________________________________________________________     2000:1 GADM/IPBC                                                               __________________________________________________________________________     Test Level                                                                           Organism                                                                            48 Hours                                                                             7 Days                                                                               14 Days                                                                              21 Days                                                                              28 Days                                     __________________________________________________________________________      0.025%                                                                              AN   300   21    10    <10   11                                           0.025%                                                                              CAN  480,000                                                                              890,000                                                                              940,000                                                                              1,040,000                                                                            130,000                                      0.025%                                                                              ECOLI                                                                               230,000                                                                              <10   <10   <10   <10                                          0.025%                                                                              PC   <10   <10   <10   <10   <10                                          0.025%                                                                              PSA  <10   <10   <10   <10   <10                                          0.025%                                                                              SA   78,000                                                                               <10   <10   <10   <10                                         0.05% AN   <10   <10   <10   <10   <10                                         0.05% CAN  110,000                                                                              4,100,000                                                                            3,600,000                                                                            330,000                                                                              97,000                                      0.05% ECOLI                                                                               120,000                                                                              <10   <10   <10   <10                                         0.05% PC   <10   <10   <10   <10   <10                                         0.05% PSA  <10   <10   <10   <10   <10                                         0.05% SA   56,000                                                                               <10   <10   <10   <10                                         0.1%  AN   <10   <10   <10   <10   <10                                         0.1%  CAN  1,200,000                                                                            53,000                                                                               430,000                                                                              144,000                                                                              110,000                                     0.1%  ECOLI                                                                               <10   <10   <10   <10   <10                                         0.1%  PC   <10   < 10  <10   <10   <10                                         0.1%  PSA  <10   <10   <10   <10   <10                                         0.1%  SA   <10   <10   <10   <10   <10                                         0.2%  AN   <10   <10   <10   <10   <10                                         0.2%  CAN  90,000                                                                               <10   <10   <10   60                                          0.2%  ECOLI                                                                               <10   <10   <10   <10   <10                                         0.2%  PC   <10   <10   <10   <10   <10                                         0.2%  PSA  <10   <10   <10   <10   <10                                         0.2%  SA   <10   <10   <10   <10   <10                                         Unpreserved control                                                            AN         50,000                                                                               33,000                                                                               33,000                                                                               13,000                                                                               5,400                                       CAN        780,000                                                                              780,000                                                                              780,000                                                                              500,000                                                                              170,000                                     ECOLI      600,000                                                                              3,100,000                                                                            920,000                                                                              920,000                                                                              140,000                                     PC         11,000,000                                                                           30,000,000                                                                           10,000,000                                                                           10,000,000                                                                           1,400,000                                   PSA        3,800 600   12,800                                                                               12,800                                                                               100,000                                     SA         14,000,000                                                                           410,000                                                                              7,100 7,100 80                                          Inoculum Concentration                                                                    0 Hours                                                                              21 Days                                                       AN         53,000                                                                               10,000                                                        CAN        1,900,000                                                                            310,000                                                       ECOLI      170,000                                                                              3,500,000                                                     PC         87,000                                                                               2,500,000                                                     PSA        390,000                                                                              5,400,000                                                     SA         200,000                                                                              4,100,000                                                     __________________________________________________________________________

Discussion of Challenge Testing Results

The 28-day challenge results reported in Tables 15-23 above demonstrate the effectiveness of the preservative admixture of the invention in a use emulsion composition against a wide range of bacteria and fungi organisms.

For example, admixture compositions of Germall® II and IPBC at a wt. ratio of 2000:1 (Table 15), when present at use levels of 0.05 to 0.2%, corresponding to 0.75 to 10 ppm IPBC and 500 to 2000 ppm methylol levels, provide substantially complete protection against all tested organisms after 28 days. At the low use level of 0.05% active, all the challenge tests passed within 21 days. Then, upon reinoculation after 21 days, all organisms died within 7 days except CAN which cleared within 14 days.

Table 21 shows the challenge test results for DMDMH and IPBC admixtures at the same 2000:1 wt. ratio. A use level of 0.2%, however is needed for this blend to pass against all organisms after 21 days. Upon reinoculation, all organisms died within 7 days with the exception of CAN which cleared within 14 days. It is thus evident from these results that Germall® II blended with IPBC is 4 times more effective than a DMDMH/IPBC blend

Germall® II also is superior to GADM as the methylol compound, as shown in Table 23.

While the invention has been described with particular reference to certain embodiments thereof, it will be understood that changes and modifications may be made which are within the skill of the art. Accordingly, it is intended to be bound only by the following claims, in which: 

What is claimed is
 1. A water soluble preservative antimicrobial composition for addition to commercial use products at predetermined use levels to provide synergistic biocidal activity against a wide range of fungi and gram-negative and gram-positive bacteria, comprising an admixture of(a) N-[1,3-bis(hydroxymethyl)-2,5-dioxo-4-imidazolidinyl]-N,N'-bis(hydroxymethyl) urea, and (b) 3-iodo-2-propynylbutyl carbamate in a weight ratio of (a):(b) of 100:1 to 2000:1.
 2. A water soluble preservative admixture according to claim 1 wherein said weight ratio is 200:1 to 500:1.
 3. A commercial use product which is protected for an extended period of time against contamination by a wide range of fungi and gram-negative and gram-positive bacteria which includes 0.01 to 0.5% by weight of the water soluble preservative concentrate of claim
 1. 4. A commercial use product according to claim 3 which includes about 0.1% by weight of the water soluble preservative concentrate of claim
 2. 5. A commercial use product according to claim 3 in which said concentrate is water solubilized and uniformly distributed throughout said composition.
 6. A commercial use product according to claim 3 in which (b) is present therein in an amount of 0.5 to 10 ppm, and (a) is present in an amount of at least 250 ppm.
 7. A commercial use product according to claim 3 which is a personal care, household or industrial composition. 